化学
钌
催化作用
光化学
分子内力
单体
氧气
钳子运动
化学计量学
过氧化氢
物理化学
立体化学
有机化学
聚合物
作者
Stephan W. Kohl,Lev Weiner,Leonid Schwartsburd,Leonid Konstantinovski,Linda J. W. Shimon,Yehoshoa Ben‐David,Mark A. Iron,David Milstein
出处
期刊:Science
[American Association for the Advancement of Science (AAAS)]
日期:2009-04-03
卷期号:324 (5923): 74-77
被引量:441
标识
DOI:10.1126/science.1168600
摘要
Discovery of an efficient artificial catalyst for the sunlight-driven splitting of water into dioxygen and dihydrogen is a major goal of renewable energy research. We describe a solution-phase reaction scheme that leads to the stoichiometric liberation of dihydrogen and dioxygen in consecutive thermal- and light-driven steps mediated by mononuclear, well-defined ruthenium complexes. The initial reaction of water at 25°C with a dearomatized ruthenium (II) [Ru(II)] pincer complex yields a monomeric aromatic Ru(II) hydrido-hydroxo complex that, on further reaction with water at 100°C, releases H 2 and forms a cis dihydroxo complex. Irradiation of this complex in the 320-to-420–nanometer range liberates oxygen and regenerates the starting hydrido-hydroxo Ru(II) complex, probably by elimination of hydrogen peroxide, which rapidly disproportionates. Isotopic labeling experiments with H 2 17 O and H 2 18 O show unequivocally that the process of oxygen–oxygen bond formation is intramolecular, establishing a previously elusive fundamental step toward dioxygen-generating homogeneous catalysis.
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